質子交換膜燃料電池電解質與電極配方與製程之研究

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詹凱愉(Kai-Yu Zhan) 查詢紙本館藏

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能源工程研究所

論文名稱

質子交換膜燃料電池電解質與電極配方與製程之研究
(Research on formulation and manufacturing process of electrolyte and electrode of proton exchange membrane fuel cell)

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至系統瀏覽論文 (2028-9-1以後開放)

摘要(中)

本研究使用脈衝雷射沉積法(Pulsed Laser Deposition, PLD)製備Pt奈米顆粒並應用於燃料電池陰陽極端之觸媒層，結合直通流道板及自製微孔層並滴塗含有二氧化鈰顆粒的Nafion薄膜(Dropcasted Nafion film)將質子交換膜直接滴塗於觸媒層上，在膜內增加質子通道，提升質子與水的傳導能力，並增加膜內保水性、降低自由基所造成的降解，提升膜的耐久性。
本研究先進行燃料電池流道結構的優化，3x3單區及三區的性能比較，並將實驗室學姊在5x5流道減薄的優化結果應用在適合脈衝雷射沉積製程的3x3流道中。減薄發泡材流場具有較寬的進出氣口可改善流體分布均勻性並降低壓降，顯示經過改良之流道，亦可有效提高電池之性能。
過去實驗室皆是使用39BC碳紙進行研究，可以適用於滴塗膜燃料電池製程，但因為目前此型號已停產，須尋找替代產品。而39BB碳紙因為裂縫較大、裂縫表面積占比較高其裂縫寬度較39BC大、裂縫表面積占比也較39BC高，經測試不適用於滴塗膜燃料電池，需自製微孔層。在成功製作出微孔層後，將造孔劑加入MPL漿料中，再利用高溫的方式，在烤乾微孔層的同時，將分布在其中的造孔劑去除，藉此留下多孔隙的結構，增進氣體傳輸效率，使得性能可以提升。
並透過比較二氧化鈰的摻雜量，在相同的操作溫度及溫度下，因二氧化鈰有好的吸水特性，使得膜能更有效的吸收水分。由於水分在膜中的分布改變，水傾向膜的方向集中，不會積聚於觸媒層，減緩觸媒層的水淹現象，可以提高電池的開路電壓及功率密度。

摘要(英)

This study employed the Pulsed Laser Deposition (PLD) method to prepare Pt nanoparticles for application in the catalyst layer of fuel cell anode and cathode. By combining a straight-through flow plate with a self-made microporous layer, a Nafion thin film containing cerium dioxide particles was drop-casted on the catalyst layer. This approach increased proton conduction and water transport within the membrane, improved water retention, and reduced degradation caused by free radicals, thereby enhancing the durability of the membrane.
In this study, the optimization of the fuel cell flow channel structure was conducted. The performance of 3x3 single-area and three-area configurations was compared. The optimization results obtained from thinning the 5x5 flow channel in a previous experiment by a senior researcher in the laboratory were applied to the 3x3 flow channel suitable for the pulsed laser deposition process. Thinning the foamed material in the flow field resulted in wider inlet and outlet openings, improving the uniformity of fluid distribution and reducing pressure drop. These modifications demonstrated the effective enhancement of the fuel cell performance.Previous studies in the lab utilized 39BC carbon paper, which was suitable for drop-casting membrane fuel cell fabrication. However, as this model is no longer in production, an alternative product needed to be identified. 39BB carbon paper had larger cracks and higher crack surface area compared to 39BC, rendering it unsuitable for drop-casting membrane fuel cells. Therefore, a self-made microporous layer was developed. After successfully fabricating the microporous layer, a pore-forming agent was added to the MPL slurry. Through a high-temperature process, the pore-forming agent was removed, leaving a porous structure that improved gas transport efficiency and enhanced performance.
Furthermore, the doping level of cerium dioxide was compared. At the same operating temperature and humidity, the good water-absorbing properties of cerium dioxide enabled the membrane to effectively absorb moisture. The change in water distribution within the membrane concentrated water towards the center, preventing flooding of the catalyst layer and improving reaction efficiency, thereby increasing the fuel cell′s current density.

關鍵字(中)

★ 脈衝雷射沉積
★ 滴塗質子交換膜
★ 二氧化鈰
★ 自製微孔層

關鍵字(英)

論文目次

目錄
中文摘要
v
Abstract vi
致謝
viii
目錄
ix
表目錄
xiii
圖目錄
xiv
1-1前言 1
1-2燃料電池介紹 3
1-2-1燃料電池種類 3
1-2-2質子交換膜燃料電池運作原理 6
1-2-3質子交換膜燃料電池組成結構 10
1-3觸媒層製程發展 21
1-3-1製備觸媒層之方式 21
1-3-2燃料電池觸媒層各製程之現況 30
1-3-3PEMFC主要發展之瓶頸 33
1-4本團隊已完成之工作 35
1-5研究動機與方向 36
第二章
文獻回顧 38
2-1質子交換膜燃料電池 38
2-2質子交換膜之研究 39
2-3金屬多孔材之研究與應用 39
2-4組裝受力對電池之影響組裝受力對電池之影響 40
2-5電化學交流阻抗分析電化學交流阻抗分析 41
2-6PEMFC觸媒研究發展觸媒研究發展 43
2-6-1Pt觸媒表面形貌及顆粒大小研究探討觸媒表面形貌及顆粒大小研究探討 43
2-7應用脈衝雷射沉積於燃料電池應用脈衝雷射沉積於燃料電池 44
2-7-1脈衝雷射沉積鉑於氣體擴散層脈衝雷射沉積鉑於氣體擴散層 44
2-8直接滴塗質子交換膜之燃料電池直接滴塗質子交換膜之燃料電池[45] 46
第三章實驗方法與設備實驗方法與設備 48
3-1實驗流程實驗流程 48
3-2實驗所需之材料實驗所需之材料 50
3-3刮刀塗佈法製備微孔層刮刀塗佈法製備微孔層 51
3-3-1微孔層漿料製備微孔層漿料製備 51
3-3-2微孔層製作微孔層製作 51
3-4脈衝雷射沉積系統脈衝雷射沉積系統(Pulsed Laser Deposition, PLD) 53
3-4-1脈衝雷射系統脈衝雷射系統架設架設 53
3-4-2奈米合金觸媒樣品製備參數奈米合金觸媒樣品製備參數 55
3-5滴塗滴塗CeO2:Nafion薄膜製備方式薄膜製備方式(Drop-cast Nafion film) 56
3-5-1Drop-cast Nafion film之溶液製備之溶液製備 56
3-5-2 2-D CNC printer for drop-casting Nafion film 57
3-6燃料電池之各元件介紹燃料電池之各元件介紹 58
3-6-1端板端板 59
3-6-2金屬流道與雙極板金屬流道與雙極板 60
3-6-3鎳金屬多孔材鎳金屬多孔材 60
3-6-4矽膠氣密墊片矽膠氣密墊片 61
3-6-5商用膜之商用膜之膜電極組製備及組裝膜電極組製備及組裝 62
3-6-6 Drop-casted Nafion film之膜電極組製備及組裝之膜電極組製備及組裝 63
3-7觸媒與觸媒與Drop-casted Nafion film檢測方式檢測方式 64
3-7-1掃描式電子顯微鏡掃描式電子顯微鏡(Scanning Electron Microscopy, SEM) 64
3-7-2能量色散能量色散 X射線譜射線譜(Energy-dispersive X-ray spectroscopy, EDS) 66
3-7-3穿透式電子顯微鏡穿透式電子顯微鏡(Transmission Electron Microscope, TEM) 67
3-8離子切割研磨機含冷凍控溫及空氣阻斷系統離子切割研磨機含冷凍控溫及空氣阻斷系統(Ion Milling with Cooling control unit and Air Protection System) 69
3-9燃料電池測試燃料電池測試 70
3-9-1測試系統介紹測試系統介紹 70
3-9-2單電池測試系統之操作程序單電池測試系統之操作程序 72
3-9-3電子阻抗頻譜測試電子阻抗頻譜測試 76
第四章實驗結果與討論實驗結果與討論 80
4-1不同流道種類對商用膜燃料電池之影響不同流道種類對商用膜燃料電池之影響 80
4-1-1單電池極化曲線測試性能比較單電池極化曲線測試性能比較 80
4-1-2不同流道種類之商用膜燃料電池之不同流道種類之商用膜燃料電池之EIS分析分析 81
4-2不同極板材料種類對商用膜燃料電池之影響不同極板材料種類對商用膜燃料電池之影響 83
4-2-1單電池極化曲線測試性能比較單電池極化曲線測試性能比較 83
4-2-2電化學交流阻抗頻譜分析電化學交流阻抗頻譜分析 85
4-3不同微孔層製程應用在滴塗膜燃料電池之影響不同微孔層製程應用在滴塗膜燃料電池之影響 86
4-3-1微孔層製程表面分布分析微孔層製程表面分布分析 86
4-3-2單電池極化曲線測試性能比較單電池極化曲線測試性能比較 89
4-3-3電化學交流阻抗頻譜分析電化學交流阻抗頻譜分析 90
4-4不同濃度二氧化鈰摻雜量對滴塗膜燃料電池之影響不同濃度二氧化鈰摻雜量對滴塗膜燃料電池之影響 92
4-4-1CeO2奈米顆粒大小奈米顆粒大小TEM影像分析影像分析 92
4-4-2Drop-cast Nafion-CeO2 film 表面分布元素分析表面分布元素分析 93
4-4-3單電池極化曲線測試性能比較單電池極化曲線測試性能比較 94
4-4-4電化學交流阻抗頻譜分析電化學交流阻抗頻譜分析 96
4-4-5 15小時開路電壓測試小時開路電壓測試 98
第五章結論結論 100
第六章未來展望未來展望 102
參考文獻 103

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指導教授

曾重仁

審核日期

2023-7-20

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